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High sensitivity glucose detection at extremely low

Cite this: RSC Adv., 2018, 8, 7942
concentrations using a MoS2-based field-effect
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transistor
Junjie Shan,a Jinhua Li, *a Xueying Chu,a Mingze Xu,a Fangjun Jin,a Xiaojun Wang,b
Li Ma,b Xuan Fang,ac Zhipeng Weic and Xiaohua Wangc

Received 23rd December 2017
Accepted 7th February 2018
DOI: 10.1039/c7ra13614e
rsc.li/rsc-advances
In recent years, molybdenum disulfide (MoS2) based field-effect transistors (FETs) have attracted much attention
because of the unique properties of MoS2 nano-materials as an ideal channel material. Using a MoS2 FET as
a glucose solution biosensor has the advantages of high sensitivity and rapid response. This paper is
concerned with the fabrication of a bilayer MoS2-based FET and the study of its application in the high
sensitivity detection of an extremely low concentration glucose solution. It was found that the source-drain
current (Ids) increases as the concentration of the glucose solution increases at the same gate voltage (Vgs)
and drain voltage (Vds). The sensitivity of the biosensor as high as 260.75 mA mM
1 has been calculated and
the detection limit of 300 nM was measured. The unknown concentration of a glucose solution was also
detected using data based on the relationship between Ids and glucose solution concentration. In addition,
many significant advantages of the biosensor were observed, such as short response time (<1 s), good
stability, wide linear detection range (300 nM to 30 mM) and the micro-detection of glucose solutions. These
unique properties make the bilayer MoS2-based FET a great potential candidate for next generation biosensors.

DNA, proteins and so on. These devices have attracted huge

Introduction
FETs are an important part of modern microelectronic tech-
nology for the advantages of high input resistance, low noise,
low power consumption, large dynamic range, easy integration,
non secondary breakdown phenomenon and wide safe working
range. The main applications of FETs are in amplied circuits,
impedance conversion, variable resistance, constant current
sources, electronic switches and so on. MoS2 is an ideal channel
material for FETs due to the small number of dangling bonds
on the surface of MoS2 and its stable structure.1–8 FETs based on
MoS2 have the advantages of high switching current ratio, high
carrier mobility and low energy dissipation, which meet the
requirements of smaller size, lower cost, less power consump-
tion, and faster computing in integrated circuits for modern
electronic products.7,8 Applications of MoS2 FETs in novel
electronic devices such as electrochemical sensors, biosensors,
solar cells, and gas sensors, have recently been reported.9,10
In recent years, the sensors based on MoS2 FETs have been
developed to detect various species such as H2O2, NO2, NH3,
a
School of Science, International Joint Research Center for Nanophotonics and
Biophotonics, Changchun University of Science and Technology, 7089 Wei-Xing
Road, Changchun 130022, P. R. China. E-mail: jhli_cust@163.com; Tel: +86 0431
85582739
b
Department of Physics, Georgia Southern University, Statesboro, GA 30460, USA
c
State Key Laboratory of High Power Semiconductor Laser, Changchun University of
Science and Technology, 7186 Wei-Xing Road, Changchun 130028, P. R. China
interest because of the advantages such as high sensitivity, low
detection limit, label free detection, low power consumption,
portability and large scale production.9,11–17 The sensor and the
test system can also be integrated on a chip to actualize the
macroscopic and fast detection of the measuring object.9,18
Relevant research shows that the sensitivity of a MoS2-based pH
sensor has been achieved as high as 59 mV per pH. Ultrasen-
sitive and specic protein sensing has also been achieved with
a sensitivity of 196 mV per pH even at 100 femtomolar
concentration.11 Zhou and his group have demonstrated the
good sensing performance of the MoS2 FET towards nitrogen
dioxide (NO2) and ammonia (NH3).9,19
Some of the salient features of 2D layered MoS2 for different
sensing applications have been researched, including the bio-
sensing, gas sensing, electrochemical sensing and SERS
sensing.9 Due to the wide application of sensitive and reliable
glucose sensing in clinical diagnosis, food analysis and
biotechnology, the development of glucose sensor has received
continuous interest.20 The detection of glucose in blood and cells
will be signicant for medical study.21 Currently, the electro-
chemistry method is mainly used for the detection of glucose
concentration.22–25 But this method requires the environment
containing a large amount of liquid, which leads the activity of
biological protein molecules to be affected seriously by temper-
ature, toxicity and pH value of the environmental. The micro-
detection of glucose solution cannot be achieved accurately
and the detection process is cumbersome and lacks stability.

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At recent reports, FET based glucose biosensor have been
successfully prepared by different channel materials, such as
carbon nanotubes, ZnO and graphene. The biosensor based on
graphene FET has a narrow linear range (3.3–10.9 mM).26 The
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effect in bilayer MoS2 for boosting the current drive of FETs.36
Moreover, the Hall mobilities increase as the density of states
increases, reaching 375 cm2 V
1 s
1 for the bilayer, in contrast
to 250 cm2 V
1 s
1 for the monolayer.37 Therefore, the bilayer

linear range can be broadened to a large extent when the
channel material is replaced by carbon nanotubes or ZnO.27,28
But their long response time of 10 s is not conducive to the
rapid and accurate concentration detection of glucose solution.
On the other hand, researchers have corroborated through
theoretical and experimental studies that the zero band gap of
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MoS2 FET based biosensor would exhibits the stable and high
sensitive responses due to the strong impact of its structure and
electrical properties.38 Unfortunately, the detection of glucose
solution based on the MoS2 FET has not been reported so far. In
our research, a biosensor based on the bilayer MoS2 back-gate
FET was fabricated successfully and the application of the

graphene limits its application in semiconductor devices.11
Contrast to graphene, the MoS2 which has the similar layered
structure to graphene shows better promising properties for
biosensors due to its non-zero band gap.3,9,29–34 The layered
MoS2 nanomaterial have been recently developed and employed
in various applications, including some new sensors because of
it layer-dependent electrical properties.9 In previous studies, Li
et al. reported the observation of thickness reduction induced
crossover of electrical contact at Au/MoS2 interfaces.35 They
found that the interfacial potential barrier can be nely tailored
from 0.3 to 0.6 eV by merely varying the thickness of MoS2. The
contact resistivity of devices slightly decreases with the reducing
of MoS2 thickness, which mainly governed by the quantum
connement effect.35 In addition, the density of states of bilayer
MoS2 nanosheet is three times higher than that of monolayer
MoS2, leading to considerably high drive currents in the
ballistic limit. The conducting channels can be created by eld
biosensor in detection of glucose concentration was demon-
strated for the rst time. We discovered that the Ids of the
biosensor increases with the increase of glucose concentration.
Through the measurements of Ids, the MoS2 FET biosensor
shown a good sensing performance. The high sensitivity of
260.75 mA mM
1 and extremely low detection limit of 300 nM
have been achieved in our researches.
Experimental section
Materials and reagents
MoS2 bulk materials (Spi, SUPPLIES), D-glucose (C6H12O6$H2O,
99.5%), Glucose oxidase (GOx, from Aspergillus niger species,
180 U mg
1). Potassium phosphate monobasic (KH2PO4, 99.5%),
potassium phosphate dibasic trihydrate (K2HPO4$3H2O, 99.0%),
potassium hexacyanoferrate (K3[Fe(CN)6]), potassium ferrocya-
nide (K4[Fe(CN)6]$3H2O).

Fig. 1 MoS2-based FET biosensor device. (a) Schematic diagram of the bilayer MoS2-based FET. (b) Optical image of the sample cell. The glucose
solution is injected into the rectangular hole of the sample cell. (c) Image of the lithography board. Four kinds of devices with different channel
widths, 2, 3, 4 and 5 mm, are included in the board. (d) The metallographic micrograph of the channel material stripped mechanically in the
channel region of (c). The length and width of the MoS2 channel are 2 and 3 mm, respectively.

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The specic preparation process of the glucose solution with

different concentrations is as follows: 80 mL of a 0.1 mol L
1
PBS solution was prepared as the solvent for the glucose solu-
tion, the PBS is a mixture of KH2PO4, K2HPO4, K3Fe(CN)6, and
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K4Fe(CN)6. The glucose of different quality was dissolved in PBS

solution to guarantee the concentration of glucose solution as
0–30 mM. Appropriate amounts of glucose oxidase (GOx) was
added to each glucose solution before testing.

Fabrication of FET based glucose biosensors

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In our study, the different concentration of glucose solution was

detected by a FET biosensor. The back-gate FET was adopted
due to the surface of channel material had to contact with the
glucose solution in the sensing process. The structure of the
MoS2 FET is shown in Fig. 1a. In addition to the FET, a sample
cell was also necessary. The sample cell which made of plex- Fig. 2 Raman spectrum of the channel material. The number of layers
iglass was designed to three parts and screwed together with the of the MoS2 nanosheet we prepared can be confirmed as bilayer. Inset,
MoS2 FET. The physical diagram of the sample cell is shown in the height gradient between the channel material and the underlying
substrate was tested by the AFM, the thickness of the MoS2 channel
Fig. 1b. In the process of testing, the glucose solution with
material is 1.36 nm.
different concentration was injected into the rectangular hole
which above the sample cell. In order to protect the channel
material, electrodes of the back-gate FET was formed on the
SiO2/Si substrate which before the MoS2 was exfoliated. The
source and drain electrodes were made of Au/Ni (70 nm/10 nm),
and the back gate electrode was made of quick-dry silver paste.
The device was placed on a square glass plate (1.5 cm  1.5 cm)
and the back-gate electrode was leaded to the glass plate. The
specic process is as follows:
The rst process is to design the board of the UV photoli-
thography which was used to prepare the source and drain
electrodes of MoS2 FET, as shown in Fig. 1c. The overlapping
areas of the gray electrode leads are the channel regions of the
FET. The channel width of the MoS2 FET was designed to 2, 3, 4
and 5 mm, respectively. The preparation of the electrodes were
carried out by the UV photolithography technique and the
electron beam (e-beam) evaporation technique on the SiO2/Si
substrate. The next procedure is to exfoliate the highly mirrored
MoS2 bulk materials in channel regions, which was shown in
Fig. 1c. Micromechanical exfoliation (Scotch-tape method) is
the traditional and the simplest technique used for the prepa-
ration of atomically thin layered 2D nanomaterials with high
quality and crystallinity.9 This technology is widely used in
preparation of the channel materials of FETs. Metallographic
micrograph of the channel material was shown in Fig. 1d, the
yellow parts were the source and drain electrode leads formed
by the e-beam deposition of 70 nm/10 nm Au/Ni, and the black
regions between the lead wires were the channel regions. The
length and width of the MoS2 channel material we prepared are
2 and 3 mm, respectively. Subsequent characterizations and
tests are all performed on this device. The nal step is the
preparation of back-gate electrode. A quick-drying silver paste Fig. 3 The basic electrical characterization of the MoS2 FET. (a) Output
was dripped on the backside of the SiO2/Si substrate. Then the characteristic curve of the device, drain current (Ids) as a function of
device was placed on a square microslide and the back-gate drain voltage (Vds) with the back gate voltage (Vgs) varying from
40 to
40 V, in a step of 5 V. (b) Transfer characteristic curve of the device, Ids
electrode of the FET was led to the surface of the microslide,
as a function of Vgs with the Vds of 0.5 V. Inset, the logarithmic image of
as shown in Fig. 1a. The three electrodes of the FET are facing transfer characteristic curve (Ids–Vgs).
upwards for subsequent tests.

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Measurements (B1500, Keysight). The data of the relationship between the Ids
and the glucose concentration was obtained and the sensitivity of
The thickness of the channel material (MoS2 nanosheet) were
the glucose biosensor was calculated.
tested by the atomic force microscope (AFM, Dimension 3100).
And the number of layers of MoS2 also been determined by
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measuring the Raman spectra (labRAM HR E, HORIBA) Results and discussion

according to the shi of the in-plane vibration mode E12g and the Basic characterization of MoS2 FET
out-plane vibration mode A1g. Then the basic electrical charac-
Characterization of the optical properties of the MoS2 by Raman
teristics of the MoS2 FET without glucose solution were tested
spectroscopy is not only fast and accurate, but also does not
before the examination of sensing performance. A suitable device
destroy the crystal structure of the sample. The number of layers
was selected as the glucose biosensor. At last, the changes of the
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of the MoS2 can be determined by measuring the Raman shi of

electrical properties of biosensor with different glucose concen-
the in-plane vibration mode E12g and the out-plane vibration
tration were measured by the semiconductor parameter analyzer
mode A1g. For instance, the Raman shi of monolayer MoS2 is

Fig. 4 MoS2 FET sensor for glucose sensing. (a) Drain current for an n-type MoS2 FET-based glucose sensor is plotted as a function of Vds for
different concentrations of the glucose solution. (b) Repeatability experiments of the glucose sensing. The even number points of glucose
concentration values are tested by the device used in the (a). (c) The real time current responses to the fluctuation of glucose concentrations. The
glucose responses for the sequential concentration increase at Vgs of 0.5 V and Vds of 2.5 V. (d) The response curve of the MoS2 FET to glucose
solution. Ids as a function of glucose concentration which is from 0 to 30 mM.

Table 1 The date of corresponding relationship between Ids and glucose concentration

Ids (mA) 0.498 0.516 0.532 0.553 0.579 0.610 0.633 0.655 0.676 0.697
Glucose (mM) 1 2 3 4 5 6 7 8 9 10
Ids (mA) 0.719 0.740 0.761 0.783 0.804 0.825 0.847 0.868 0.889 0.911
Glucose (mM) 11 12 13 14 15 16 17 18 19 20
Ids (mA) 0.932 0.953 0.974 0.996 1.021 1.043 1.062 1.084 1.107 1.129
Glucose (mM) 21 22 23 24 25 26 27 28 29 30

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16–18 cm
1; the Raman shi of bilayer and trilayer MoS2 are
21 cm
1 and 23 cm
1, respectively.39–43 The testing results of
Raman spectroscopy shown that the Raman shi of MoS2 is
20.4 cm
1 with the excitation of the 532 nm laser, as shown in
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Fig. 2. It can be inferred that the channel material we prepared

is the bilayer MoS2 nanosheet. In addition, the height gradient
between the channel material and the underlying substrate was
tested by the AFM, as shown in Fig. 2 inset. The test results
shown that the thickness of the MoS2 channel material is
1.36 nm, it also validated the Raman data of the bilayer MoS2 we
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have tested.
The electrical characteristics of the MoS2 FET have a strong
impact on the sensitivity of the biosensor. The testing of the
electrical properties of the MoS2 nanosheet based FET without
glucose solution is shown in Fig. 3. As the output characteristic
(Ids–Vds) curve shown in Fig. 3a, the Ids increases with the
increase of Vds. Especially in the low voltage region of Vds, it can
be observed that the Ids increases linearly with Vds and the curve
pass through the original point, indicating that the good ohmic
contact was formed between the electrodes and MoS2 layers,
which is benecial to the injection of electrons. The device can
be effectively controlled by the Vgs, which is illustrated by the
output characteristic curve of the device with different Vgs in
Fig. 3a; several important electrical parameters of MoS2 FET can
be achieved from the transfer characteristic curve (Ids–Vgs) and
the logarithmic image of Ids–Vgs, which was shown in Fig. 3b
and its illustrations. According to calculation results: the eld-
effect mobility (m) reached 33.5 cm2 V
1 s
1, the trans-
conductance (gm) was 1.7 and the switching current ratio
(Ion/Ioff) was as high as 106.
Fig. 5 MoS2 FET sensor for ultra low concentration glucose sensing.
(a) The detection limit of the biosensor based on MoS2 FET observed
Detection of glucose using MoS2 FET based biosensor by the output characteristic curve is 300 nM. (b) Drain current as
a function of glucose concentration which ranges from 0 to 1 mM at Vgs
In the research of glucose sensing performance, the output of 0.5 V and Vds of 2.5 V. By calculation, the sensitivity of our biosensor
characteristic curves were tested with the different glucose has been achieved as high as 260.75 mA mM
1.
concentration. Fig. 4a shown the Ids of MoS2 FET varies with the
concentration of glucose solution. This phenomenon can be
explained by the enzymatic reaction of glucose with GOx and The repeatability experiments were carried out by the same
formation of the products.44 The underlaying sensing mecha- device and under the same conditions aer 45 days. The device
nism of the glucose biosensor based on bilayer MoS2 FET is was used to test the even number points of glucose concentra-
attributed to the reaction of H2O2 generated by the oxidation of tion values, as shown in Fig. 4b. The results shown that the
glucose. The details is that the glucose solution can generate device has a good stability. The real time sensor response to the
gluconate and hydrogen peroxide (H2O2) aer being catalyzed addition of different concentration of glucose was shown in the
by the glucose oxidase (GOx), and H2O2 will be dissociated and Fig. 4c. The test was started with a pure PBS solution under xed
produce hydrogen ions (H+) and electrons (e
). The concentra- Vds of 2.5 V and Vgs of 0.5 V. 1 mM glucose solution was rst
tion of electrons increases on the surface of conductive channel injected at 180 s. And then, the glucose solution with higher
of the device with the process of enzymatic reaction. And the concentrations were replaced the last one ever minute there-
conductance of the channel material is increased because the aer. The relationship between glucose concentration and the
MoS2 is a n-type semiconductor. This is due to the n-doping electrical parameters of MoS2 FET were shown in Fig. 4d. Then
effect resulting from the direct electron transfer on the the unknown concentrations of glucose solution can be detec-
surface of the MoS2 nanosheet. There would be a charge ted by the Ids of the MoS2 FET (Vgs of 0.5 V, Vds of 2.5 V), as
transfer from the H2O2 molecules to the MoS2 channel.26,27,44–49 illustrated in Table 1.
The glucose oxidation reaction is as follows:
GOx
D-Glucose þ H2 O þ O2 ƒƒƒƒƒ!D-gluconic acid þ H2 O2 Sensitivity test
H2 O2 /O2 þ 2Hþ þ 2e

In order to research the detection limit and the sensitivity of the
MoS2 FET based biosensor, the glucose solution with extremely

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Table 2 Analytical features of some reported for glucose biosensors based on the FETa

Response
Modied surface Sensitivity LDR DL time Reference
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CPNTs nr 0.5–20 mM nr 5–10 s Yoon et al. (2008)

Graphene nr 3.3–10.9 mM 3.3 mM nr Kwak et al. (2012)
Graphene 0.4086 mA mM
1 1.25–10 mM 1.25 mM nr Cagang et al. (2016)
Graphene 2.5 mA mM
1 0.1–10 mM 0.1 mM nr You and Pak (2014)
rGO/C-PPy NT nr nr 1 nM <1 s Park et al. (2015)
SGGT 17.3 mV M
1 0.5–300 mM 0.5 mM nr Zhang et al. (2014)
ZnO NRs 10 mA cm
2 mM
1 0.001–45 mM 1 mM nr Ahmada et al. (2013)
0.302 mV mg
1 dl
1 60–360 mg dl
1 60 mg dL
1
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CNTFs nr Tsai et al. (2013)

ZnO NRs 38.9 mA mM
1 800 nM to 25 mM 800 nM nr Lee and Chiu (2015)
ZnO nr 1–100 mM 1 mM <0.1 s Ali et al. (2009)
ZnO 2.7 A mM
1 10–30 mM nr 20 s Yano et al. (2012)
MWCNTCOOH/PAN nr 0.005–50 mM 0.5 mM 10 s Fathollahzadeh et al. (2016b)
Bilayer MoS2 260.75 mA mM
1 300 nM to 30 mM 300 nM <1 s Our research
a
LDR, linear dynamic range; DL, detection limit; CPNTs, carboxylated polypyrrole nanotubes; rGO/C-PPy NT, reduced graphene oxide/carboxylated
polypyrrole nanotube; SGGT, solution gated graphene transistors; ZnO NRs, ZnO nanorods; CNTFs, carbon nanotube thin lms; MWCNTCOOH/
PAN, multi-walled carbon nanotubes-polyaniline nanocomposite; nr, not reported.

low concentration which from 0 nM to 1 mM was detected by the
change of output characteristic curves, as shown in Fig. 5a.
The detection limit of our biosensor is 300 nM. The Ids as
a function of glucose concentration was shown in Fig. 5b. The
sensitivity of the glucose biosensor can be calculated as high as
260.75 mA mM
1. And the response time (<1 s) and the linear
regions (300 nM to 30 mM) were tested in our experiments.
Analytical features of some reported for glucose biosensors
based on the FET are summarized in the Table 2 and compared
with those parameters obtained from our results using bilayer
MoS2 FET. As shown in Table 2, the proposed ZnO-based
glucose biosensor shown higher sensitivity,28 shorter response
time45 and wider linear dynamic range50 than those previous
reports.26,27,46,47,51–55 And the detection limit of the reduced gra-
phene oxide/carboxylated polypyrrole nanotube (rGO/C-PPy NT)
FET based biosensor42 was better than other glucose biosen-
sors.26–28,45–47,50–55 Compared with previous researches, the
bilayer MoS2-based FET we prepared show signicant advan-
tages in high sensitivity detection of extremely low concentra-
tion glucose solution.
a new path for the applications about the MoS2 FET. In practical
sensing applications, we can design a bio-integrated circuit
which contains a FET, an operational amplier, a comparator
and an LED to achieve the macroscopic, fast detection. That can
be used to realize the miniaturization and real-time detection of
human blood glucose concentration in the future.
Conflicts of interest
There are no conicts to declare.
Acknowledgements
This work is supported by the “111” Project of China (D17017),
the National Natural Science Foundation of China (21703017,
11674038, 61404009), the Advance Research Project of Weapon
and Equipment (61404140201), the Project of Education
Department of Jilin Province (JJKH20170611KJ), and the
Developing Project of Science and Technology of Jilin Province
(20160520117JH).

Conclusions
References
In summary, a biosensor based on the bilayer MoS2 back-gate
FET was fabricated and demonstrated for glucose detection
successfully in our research. In particular, the glucose concen-
tration was detected by the MoS2 FET for the rst time.
Considering the concentration of the fasting blood ranges from
3.9 to 6.1 mM, the concentration was detected in the range of 0–
30 mM by the glucose biosensor we prepared. Through
measurements of the Ids, the fabricated MoS2 FET biosensor
shown a good sensing performance. The high sensitivity of
260.75 mA mM
1 was achieved for the detection of glucose
solution which has the extremely low concentration level (300
nM). The other advantages of our biosensor such as short
response time (<1 s), good stability, small size and trace detec-
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